Thermal Stability of Colloidal InP Nanocrystals: Small Inorganic Ligands Boost High-Temperature Photoluminescence

Rowland, Clare E.; Liu, Wenyong; Hannah, Daniel C.; Chan, Maria K. Y.; Talapin, Dmitri V.; Schaller, Richard D.

doi:10.1021/nn405811p

Cited by 59 publications

(76 citation statements)

References 38 publications

(61 reference statements)

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“…In the study of Wang et al, the authors observed significantly improved stability with the additional silica‐coated core/shell NCs. When they performed temperature stability test with the pristine core/shell NCs, their core/shell NCs can retain only 61% of their initial emission at 473 K and almost quenched emission at 573 K . Regarding the InP based QDs, in their work the authors studied the thermal stability of InP/ZnS up to 800 K and the results demonstrated that integrated PL of these NCs decreased to almost 10% of their initial value at around 500 K .…”

Section: Resultsmentioning

confidence: 64%

Highly Stable, Near‐Unity Efficiency Atomically Flat Semiconductor Nanocrystals of CdSe/ZnS Hetero‐Nanoplatelets Enabled by ZnS‐Shell Hot‐Injection Growth

Altıntas

Quliyeva

Gungor

et al. 2019

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128

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Colloidal semiconductor nanoplatelets (NPLs) offer important benefits in nanocrystal optoelectronics with their unique excitonic properties. For NPLs, colloidal atomic layer deposition (c‐ALD) provides the ability to produce their core/shell heterostructures. However, as c‐ALD takes place at room temperature, this technique allows for only limited stability and low quantum yield. Here, highly stable, near‐unity efficiency CdSe/ZnS NPLs are shown using hot‐injection (HI) shell growth performed at 573 K, enabling routinely reproducible quantum yields up to 98%. These CdSe/ZnS HI‐shell hetero‐NPLs fully recover their initial photoluminescence (PL) intensity in solution after a heating cycle from 300 to 525 K under inert gas atmosphere, and their solid films exhibit 100% recovery of their initial PL intensity after a heating cycle up to 400 K under ambient atmosphere, by far outperforming the control group of c‐ALD shell‐coated CdSe/ZnS NPLs, which can sustain only 20% of their PL. In optical gain measurements, these core/HI‐shell NPLs exhibit ultralow gain thresholds reaching ≈7 µJ cm−2. Despite being annealed at 500 K, these ZnS‐HI‐shell NPLs possess low gain thresholds as small as 25 µJ cm−2. These findings indicate that the proposed 573 K HI‐shell‐grown CdSe/ZnS NPLs hold great promise for extraordinarily high performance in nanocrystal optoelectronics.

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Section: Resultsmentioning

confidence: 64%

Highly Stable, Near‐Unity Efficiency Atomically Flat Semiconductor Nanocrystals of CdSe/ZnS Hetero‐Nanoplatelets Enabled by ZnS‐Shell Hot‐Injection Growth

Altıntas

Quliyeva

Gungor

et al. 2019

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128

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“…1 We found that the oleic acid capped CdSe/CdS NCs that were also made by high-temperature seeded growth 28 performed similarly to phosphonatecapped NR heterostructures ( Figure S4), indicating that at least among organic ligands the PL behavior is not affected by the ligand on the particles. However, we did not test an inorganic ligand, and we did not heat the samples above 600 K, situations in which it is possible that conclusions could be different.…”

Section: Articlementioning

confidence: 81%

High-Temperature Photoluminescence of CdSe/CdS Core/Shell Nanoheterostructures

Diroll

Murray

2014

ACS Nano

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The steady-state and time-resolved photoluminescence properties of CdSe/CdS heterostructures are studied as a function of temperature from 300 to 600 K. The emission properties of samples are found to behave similarly to bulk CdSe, with the samples maintaining high color purity and a slightly contracting band gap at elevated temperature. Photoluminescence from CdSe/CdS samples is maintained with high stability over prolonged illumination and multiple heating and cooling cycles. Structures synthesized with variation in the core and the shell dimensions show that the preservation of emission intensity at high temperature depends strongly on the microscopic structure of the samples. For samples synthesized by seeded growth, the size of the CdSe core is highly correlated with the fraction of preserved sample photoluminescence intensity at high temperature. Temperature-dependent lifetime data suggest that the core structure predicts the stability of photoluminescence at elevated temperatures by controlling the radiative rate. The rate of electron capture, for which the volume fraction of the core is a structural proxy, underpins the ability for radiative processes to compete with thermally induced nonradiative decay pathways. Heterostructures synthesized below 200 °C using highly reactive organometallic precursors show markedly lower thermal stability than samples prepared by seeded growth at 360 °C, suggesting that the temperature of nanocrystal synthesis has direct consequences for the thermal stability of photoluminescence.

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“…208 In this regard, the PL temperature-dependence of InP/ZnS QDs has been investigated, [209][210][211] where the improved performance of the coreshell system over core-only InP was attributed to reduced electron trapping on the surface. 210 In addition to core-shell heterostructures, replacing long organic ligands on core-only InP with short inorganic ligands (S 2À as well as Sn 2 S 6 4À ), resulted in similar thermal stability, including PL recovery in cycling between 300 and 800 K. 210 …”

Section: Phosphors For Lightingmentioning

confidence: 99%

A sustainable future for photonic colloidal nanocrystals

2015

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Colloidal nanocrystals - produced in a growing variety of shapes, sizes and compositions - are rapidly developing into a new generation of photonic materials, spanning light emitting as well as energy harvesting applications. Precise tailoring of their optoelectronic properties enables them to satisfy disparate application-specific requirements. However, the presence of toxic heavy metals such as cadmium and lead in some of the most mature nanocrystals is a serious drawback which may ultimately preclude their use in consumer applications. Although the pursuit of non-toxic alternatives has occurred in parallel to the well-developed Cd- and Pb-based nanocrystals, synthetic challenges have, until recently, curbed progress. In this review, we highlight recent advances in the development of heavy-metal-free nanocrystals within the context of specific photonic applications. We also describe strategies to transfer some of the advantageous nanocrystal features such as shape control to non-toxic materials. Finally, we present recent developments that have the potential to make substantial impacts on the quest to attain a balance between performance and sustainability in photonics.

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Thermal Stability of Colloidal InP Nanocrystals: Small Inorganic Ligands Boost High-Temperature Photoluminescence

Cited by 59 publications

References 38 publications

Highly Stable, Near‐Unity Efficiency Atomically Flat Semiconductor Nanocrystals of CdSe/ZnS Hetero‐Nanoplatelets Enabled by ZnS‐Shell Hot‐Injection Growth

Highly Stable, Near‐Unity Efficiency Atomically Flat Semiconductor Nanocrystals of CdSe/ZnS Hetero‐Nanoplatelets Enabled by ZnS‐Shell Hot‐Injection Growth

High-Temperature Photoluminescence of CdSe/CdS Core/Shell Nanoheterostructures

A sustainable future for photonic colloidal nanocrystals

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